Small, Год журнала: 2024, Номер 20(47)
Опубликована: Авг. 15, 2024
Photocatalytic H
Язык: Английский
Angewandte Chemie International Edition, Год журнала: 2024, Номер 63(20)
Опубликована: Фев. 26, 2024
Abstract The catalytic performance for electrocatalytic CO 2 reduction reaction (CO RR) depends on the binding strength of reactants and intermediates. Covalent organic frameworks (COFs) have been adopted to catalyze RR, their abilities are tuned via constructing donor‐acceptor (DA) systems. However, most DA COFs single donor acceptor units, which caused wide‐range but lacking accuracy in modulating More elaborate regulation interactions with intermediates necessary challenge construct high‐efficiency catalysts. Herein, three‐component COF D‐A‐A units was first constructed by introducing electron‐rich diarylamine unit, electron‐deficient benzothiazole Co‐porphyrin units. Compared two‐component COFs, designed exhibit elevated electronic conductivity, enhanced reducibility, high efficiency charge transfer, further improving RR faradic 97.2 % at −0.8 V activity partial current density 27.85 mA cm −2 −1.0 exceed other COFs. Theoretical calculations demonstrate that sites suitable ability intermediates, benefit formation *COOH desorption *CO. This work offers valuable insights advancement multi‐component enabling modulated transfer improve activity.
Язык: Английский
Процитировано
22
Journal of the American Chemical Society, Год журнала: 2024, Номер 146(12), С. 8407 - 8416
Опубликована: Март 14, 2024
Although a variety of chiral porous framework materials have been reported, there are few examples known to combine molecular chirality, helicity, and three-dimensional (3D) intrinsically topology in one structure, which is beneficial for chirality transfer amplification. Here, we report the synthesis first two 3D covalent organic frameworks (COFs) with an intrinsic
Язык: Английский
Процитировано
20
Journal of the American Chemical Society, Год журнала: 2024, Номер 146(29), С. 19680 - 19685
Опубликована: Июль 9, 2024
The pore shapes of two-dimensional covalent organic frameworks (2D COFs) significantly limit their practical applications in separation and catalysis. Although various 2D COFs with polygonal pores have been well developed, constructing pentagonal remains an enormous challenge. In this work, we developed one kind the
Язык: Английский
Процитировано
19
Nature Protocols, Год журнала: 2024, Номер 19(12), С. 3489 - 3519
Опубликована: Авг. 7, 2024
Язык: Английский
Процитировано
11
Angewandte Chemie International Edition, Год журнала: 2024, Номер 63(33)
Опубликована: Июнь 6, 2024
Abstract Proton conduction is important in both fundamental research and technological development. Here we report designed synthesis of crystalline porous covalent organic frameworks as a new platform for high‐rate anhydrous proton conduction. By developing nanochannels with different topologies pathways loading neat phosphoric acid to construct robust carrier networks the pores, found that pore topology crucial Its effect on increasing conductivity an exponential mode other than linear fashion, endowing materials exceptional conductivities exceeding 10 −2 S cm −1 over broad range temperature low activation energy barrier down 0.24 eV. Remarkably, size controls mechanism, where mesopores promote via fast‐hopping while micropores follow sluggish vehicle process. Notably, decreasing content drastically reduces greatly increases barrier, emphasizing pivotal role well‐developed network transport. These findings insights unveil general transformative guidance designing framework systems ion conduction, storage, conversion.
Язык: Английский
Процитировано
9
Advanced Materials, Год журнала: 2024, Номер 36(41)
Опубликована: Авг. 19, 2024
Abstract This review focuses on the mechanism and driving force in intractable gas separation using porous adsorbents. A variety of mixtures have been discussed, including air separation, carbon capture, hydrocarbon purification. Moreover, systems are categorized according to distinctly biased modes depending minor differences kinetic diameter, dipole/quadruple moment, polarizability adsorbates, or sorted by varied occasions (e.g., CO 2 capture from flue air) forces (thermodynamic molecular sieving). Each section highlights functionalization strategies for materials, like synthesis condition optimization organic group modifications cation exchange heteroatom doping zeolites, metal node‐organic ligand adjustments MOFs. These subsequently associated with enhanced adsorption performances (capacity, selectivity, structural/thermal stability, moisture resistance, etc.) toward analog mixtures. Finally, this also discusses future challenges prospects materials separation. Therein, combination theoretical calculation parameters adsorbents may great potential, given its fast targeting candidate deeper insights into confined pores cages.
Язык: Английский
Процитировано
8
Molecules, Год журнала: 2024, Номер 29(16), С. 3916 - 3916
Опубликована: Авг. 19, 2024
The field of carborane research has witnessed continuous development, leading to the construction and development a diverse range crystalline porous materials for various applications. Moreover, innovative synthetic approaches are expanding in this field. Since first report carborane-based (CCPMs) 2007, synthesis ligands, particularly through methods, consistently posed significant challenge discovering new structures CCPMs. This paper provides comprehensive summary recent advances CCPMs, along with their applications different domains. primary challenges future opportunities expected stimulate further multidisciplinary
Язык: Английский
Процитировано
7
Angewandte Chemie, Год журнала: 2024, Номер 136(20)
Опубликована: Фев. 26, 2024
Abstract The catalytic performance for electrocatalytic CO 2 reduction reaction (CO RR) depends on the binding strength of reactants and intermediates. Covalent organic frameworks (COFs) have been adopted to catalyze RR, their abilities are tuned via constructing donor‐acceptor (DA) systems. However, most DA COFs single donor acceptor units, which caused wide‐range but lacking accuracy in modulating More elaborate regulation interactions with intermediates necessary challenge construct high‐efficiency catalysts. Herein, three‐component COF D‐A‐A units was first constructed by introducing electron‐rich diarylamine unit, electron‐deficient benzothiazole Co‐porphyrin units. Compared two‐component COFs, designed exhibit elevated electronic conductivity, enhanced reducibility, high efficiency charge transfer, further improving RR faradic 97.2 % at −0.8 V activity partial current density 27.85 mA cm −2 −1.0 exceed other COFs. Theoretical calculations demonstrate that sites suitable ability intermediates, benefit formation *COOH desorption *CO. This work offers valuable insights advancement multi‐component enabling modulated transfer improve activity.
Язык: Английский
Процитировано
4
Angewandte Chemie International Edition, Год журнала: 2024, Номер 63(45)
Опубликована: Июль 18, 2024
Abstract Helicenes represent a class of fascinating π compounds with fused yet folded backbones. Despite their broad structural diversity, harnessing helicenes to develop well‐defined materials is still formidable challenge. Here we report the synthesis crystalline porous helicene by exploring synthesize covalent 2D lattices and layered frameworks. Topology‐directed polymerization [6]helicenes porphyrin creates networks alternate helicene‐porphyrin alignment along x y directions at 1.5‐nm interval develops [6]helicene frameworks through reversed anti‐AA stack z direction form segregated columnar arrays. Notably, this configuration enables be highly red luminescent benchmark quantum yields. The trigger effieicnt intra‐framework singlet‐to‐singlet state energy transfer from facilitate intermolecular triplet‐to‐triplet molecular oxygen produce reactive species, harvesting wide range photons ultraviolet near‐infrared regions for light emitting photo‐to‐chemical conversion. This study introduces new family extended frameworks, laying groundwork unprecedented structures functions.
Язык: Английский
Процитировано
4
Journal of the American Chemical Society, Год журнала: 2025, Номер unknown
Опубликована: Фев. 8, 2025
The diversity of covalent organic frameworks (COFs) is continuously expanding, providing various materials with tailor-made structures and properties. However, the development crystalline three-dimensional (3D) COFs new topologies an essential but arduous challenge. In this study, we first developed one kind 3D lil topological structure, which were assembled by D4h- C2h-symmetric building blocks. determined in a space group Imma, each D4h-symmetric unit connected four units, forming noninterpenetrated network. densely packed copper phthalocyanine stable polyimide linkage render these as polymeric material high dielectric constant low loss at frequencies (>1 kHz). Significantly, was 63, constitutes record value among phthalocyanine-based polymers. Therefore, study not only provides important guidance for design lil-net also supplies promising application high-energy-density pulsed capacitors.
Язык: Английский
Процитировано
0